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COMPARATIVE ANALYSIS OF RADIATION CHARACTERISTICS

FROM VARIOUS TYPES OF SPENT NUCLEAR FUEL

E.F.Kryuchkov, V.A.Opalovsky, G.V.Tikhomirov

Moscow Engineering Physics Institute (State University), Russia

Abstract

At the present time, in purposes of the most effective utilization of nuclear materials, new
advanced fuel cycles are under development. These cycles imply application of uranium-plutonium,
uranium-thorium and some other types of nuclear fuel. However, it is obvious the parameters of new
nuclear fuel (NF) types will be quite different from those for traditional NF types. These differences
can affect significantly the conditions for storage, transportation and reprocessing of spent nuclear
fuel (SNF). So, it is necessary to carry out a comparative analysis of radiation characteristics for
various NF types at different stages of nuclear fuel cycle (NFC). The present paper addresses
radiation properties of the following NF types: UO2, UO2–PuO2, ThO2–PaO2–UO2. Numerical studies
have been carried out to determine radiation properties of these NF types at the following NFC stages:
radiation properties of NF directly before and after irradiation in the reactor core, after different
cooling time, radiation properties of uranium and plutonium fractions after chemical separation,
radiation properties of NF refabricated for recycle, radiation properties of NF after the second and
third recycles. The computer code package SCALE is used for evaluating the radiation properties of
different SNF types.
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Introduction

Operation of power nuclear reactors leads to SNF generation. There are two basic strategies of
SNF management: SNF disposal or repeated utilization of SNF. In both cases, an urgent necessity
arises to study radiation properties of SNF. Information about radiation properties of SNF is required
at all stages of SNF management: SNF storage in interim cooling ponds at nuclear power plants
(NPP), after SNF discharge from the reactor core, under SNF transportation, under radiochemical and
metallurgical SNF reprocessing, under long-term disposal of SNF.

The purposes of the present study are as follows:

1. comparative analysis of radiation situation around the transport container [1] with different SNF
types;
2. evaluation of contributions from different isotopes to total SNF activity.

The following NF types are analysed: the fuel composition ThO2–PaO2–UO2 [2] developed for
achieving high fuel burn-up, mixed uranium-plutonium dioxide fuel (MOX–fuel, UO2–PuO2) and, for
comparison, traditional uranium dioxide fuel (UOX-fuel). Radiation properties of all the NF types
mentioned above are determined by computations with application of the computer code package
SCALE 4.3 [3].

Radiation background of SNF

After irradiation in the reactor core, NF is characterized by high radiation background [4]. Above
600 different isotopes contribute to total SNF activity [5]. However, only some of them give definitive
contributions. Determination of the isotopes - main contributors to SNF activity for different SNF
types will allow to create an adequate mathematical model of SNF radiation source for different
purposes and to analyse an accuracy of the applied mathematical models.

Within the frames of the present study the calculations are carried out to determine activities of
irradiated fuel assemblies (FA) containing different NF types and to identify the main isotopes -
sources of these activities.

Four types of radioactivity ( α -, β -, γ - and neutron activity) are usually studied. However, such
a structure is not effective for resolving the problems set in the present study. We do not consider
alpha- and beta-radiation because of low penetrability. These types of radiation are not able to go
outside of the transport container. Two-level structure is used for analysis of gamma- and neutron
radiation.

The first level implies division of all radioactive isotopes into two fractions: heavy nuclides and
fission products. These fractions will be studied separately. It may be argued, for example, by the fact
that heavy nuclides (actinides and their decay products) and fission products (mainly, rare-earth
elements) are quite different from chemical point of view. So, there are quite different technologies
for handling with these fractions at SNF reprocessing plants. In addition, fission products (with some
exceptions) may be regarded as radioactive wastes. At the same time, some actinides can be
repeatedly utilized in NFC.

At the second level, the following radiation types are analysed: gamma-radiation, neutron
radiation generated in spontaneous fission reactions of heavy nuclides, neutron radiation generated in
(α , n ) -reactions. For fission products, gamma-radiation is the only radiation type under analysis.
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The following approach is proposed. Radioactive source can be considered as the source modeled
properly if the group of radioactive isotopes chosen for specified SNF type meets the following
requirements:

1. The isotopes with the largest activities should be chosen.

2. Summed up contribution of these isotopes to total activity of specified type should exceed
90% (in ideal case, 99,9%).
3. Each of three radiation types to be analysed should be described by, at least, two isotopes.
Also, it would be convenient if the number of significant isotopes for each radiation type
would not exceed ten.
4. If the required 90% of total activity are obtained under the number of significant isotopes
below 10 and there are else isotopes with activities of close level, then these additional
isotopes should be taken into account too.
5. Isotopic selection at different moments of SNF cooling time should be made taking into
consideration that set of the isotopes which give a main contribution to radiation background
can be changed with time.

According to these requirements, the following SNF types are analysed:

1. Traditional NF type (UO2 enriched up to 4,4% 235U). Fuel life-time consists of three
irradiation cycles (305,9 effective full power days each). Outage for refueling - 48 days.
Cooling time after fuel irradiation - 3 years. Value of fuel burn-up - 40,48 GWd/t U[3].
2. MOX-fuel (UO2+PuO2 containing 7% of reactor-grade plutonium). Depleted uranium and
plutonium produced after SNF reprocessing (SNF from item 1) are used. Irradiation
conditions are the same as those in item 1. Conditional designation - MOX1.
3. MOX-fuel (UO2+PuO2 containing 7% of reactor-grade plutonium). Depleted uranium and
plutonium produced after SNF reprocessing (SNF from item 2) are used. Irradiation
conditions are the same as those in item 1. Conditional designation - MOX2.
4. NF composition ThO2–PaO2–UO2 [2] developed for achieving ultra-high fuel burn-up. The
fuel composition includes 232Th– 69%, 231Pa–15%, 233U–16%. Irradiation conditions are the
same as those in item 1. Value of fuel burn-up - 34,12 GWd/t U.
5. NF composition ThO2–PaO2–UO2 [2] developed for achieving ultra-high fuel burn-up. The
fuel composition includes 232Th– 69%, 231Pa–15%, 233U–16%. Fuel life-time consists of thirty
irradiation cycles (305,9 effective full power days each). Outage for refueling - 48 days.
Cooling time after fuel irradiation - 10 years. Value of fuel burn-up - 341,2 GWd/t U.

Parameters of VVER-1000 (as the most widely spread reactor type in Russia [6]) are used in all
the calculations. FA of VVER-1000 represents a hexagonal prism (key size of the prism base - 23,4
cm, height of active part - 353 cm). FA contains 312 fuel rods (total uranium dioxide mass - 488 kg,
total uranium mass - 429 kg). Fuel rods are located in nodes of hexagonal lattice. Under nominal
operation regime, mean specific power generation in fuel - 44 kW/kg U [4].

Heavy nuclides, main contributors to SNF activity

Data on three activity types (neutron radiation generated in spontaneous fission reactions of
heavy nuclides (SF n), neutron radiation generated in (α , n ) -reactions and gamma-radiation, γ ) are
presented in Tables 1-3. SNF type is identified in column 1. The first figure of the second column -
irradiation time (years), the second figure - cooling time (years). The third column - activity (in
relative units). Uranium dioxide activity after 3-year irradiation time and 3-year cooling time is
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adopted as a relative activity unit. Values of activity are normalized per one FA. The fourth column
identifies the isotopes which give the largest contributions to total activity (in percents). These
isotopes are presented in order of the reducing significance. The fifth column shows total contribution
of the isotopes listed above (in percents).

Table 1. Main heavy nuclides which contribute to neutron generation in spontaneous fission
reactions.

SF n
UO2 3-0 1,88E+00 Cm242(63) , Cm244(36) 99,0
3-3 1,00E+00 Cm244(94), Pu240(3,5), Cm242(1,8), Pu242(0,6) 99,9
MOX 3-0 3,43E+01 Cm242(54), Cm244(45,9) 99,9
3-3 1,44E+01 Cm244(97), Cm242(1,3), Cm246(0,5) 98,8
MOX2 3-0 4,50E+01 Cm244(52), Cm242(47) 99,0
3-3 2,14E+01 Cm244(98), Cm242(1), Cm246(0,6), Cf252(0,3) 99,9
(Th-Pa- 3-0 7,34E-05 U232(98), Pa231(1,6) 99,6
U)O2
3-3 7,16E-05 U232(98), Pa231(1,7) 99,7
30-0 3,37E+00 Cf252(81), Cm244(17) 98,0
30-10 6,21E-01 Cm244(62), Cf252(32), Cm246(4) 98,0

Table 2. Main heavy nuclides which contribute to neutron generation in ( α -n)-reactions.

α -n
UO2 3-0 8,30E+00 Cm (90),Pu (5,1), Cm244(2), Pu239(1,4), Pu240(1,3)
242 238
99,8
3-3 1,00E+00 Pu238(41),Am241(18), Cm244(13), Pu239(11), Pu240(9,8) 92,8
MOX 3-0 1,88E+02 Cm242(94), Cm244(3), Pu238(2) 99,0
3-3 1,31E+01 Cm244(40), Pu238(34), Cm242(14), Am241(8), Pu240(2) 98,0
MOX2 3-0 2,20E+02 Cm242(93), Cm244(3,9), Pu238(3) 99,9
3-3 1,87E+01 Cm244(41), Pu238(38), Cm242(11), Pu240(2) 92,0
(Th-Pa- 3-0 2,90E+02 Po212(24), U232(20), Po216(18), Rn220(15), Ra224(10), Th228(8,8), 90,4
U)O2 Bi212(4,6)
3-3 5,00E+02 Po212(26), Po216(20), Rn220(16), Ra224(11), U232(11), Th228(10) 94,0
30-0 6,56E+01 Po212(27), Po216(21), Rn220(17), Ra224(12), Th228(10), Bi212(5,3), 97,4
U232(3), Pu238(1,6), Cm242(0,5)
30-10 2,29E+01 Po212(25), Po216(19), Rn220(15), Ra224(11), Th228(9,1), U232(7,8), 95,6
Bi212(4,6), Pu238(4,1)
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Table 3. Main heavy nuclides which contribute to generation of gamma-rays.

γ
UO2 3-0 3,45E+02 Np (41), U (2), Np238(0,6)
239 237
43,6
3-3 1,00E+00 Pu241(97), Pu238(1,3), Am241(0,5), Pu239(0,4), Pu240(0,4) Cm244(0,3) 99,9
MOX 3-0 3,27E+02 Np239(42), Pu243(3), Am242(3), Cm242(2,5), U237(2,2), Pu241(2), 55,7
Np238(1)
3-3 6,01E+00 Pu241(88), Pu238(4,5), Cm244(4,3) 96,8
MOX2 3-0 3,54E+02 Np239(41), Pu243(4,6), Am242(3,1), Cm242(2,5), U237(2,1), Pu241(1,8), 56,1
Np238(1)
3-3 6,65E+00 Pu241(84), Pu238(6,6), Cm244(5,8), Cm242(1,3), Am241(1), Pu240(0,4) 99,1
(Th-Pa- 3-0 3,21E+02 Pa233(18), U232(1,2), Pb212(0,5), Bi212(0,5), Po216(0,5), Rn220(0,5), 22,2
U)O2 Ra224(0,5), Th228(0,5)
3-3 2,52E+01 U232(15), Pb212(12), Bi212(12), Po216(12), Rn220(12),Ra224(12), 96,0
Th228(12), Po212(8)
30-0 4,48E+02 Pa233(45), U237(1,6), Np238(1,4) 48,0
30-10 1,17E+00 Pb212(11), Bi212(11), Po216(11), Rn220(11), Ra224(11), Th228(11), 93,4
U232(10), Po212(7,2), Pu238(4,9), Tl208(4,1), Pu241(1,3)

Table 4. Ratio of neutron activity generated in spontaneous fission reactions and in ( α -n)-
reactions to gamma-activity of heavy nuclides (for uranium fuel and uranium-plutonium fuel).

SNF SFn / γ (α − n ) / γ
UO2 –3– 0 3,71E-10 3,41E-11
UO2 –3– 3 6,81E-08 1,42E-09
MOX –3– 0 7,15E-09 8,16E-10
MOX –3– 3 1,63E-07 3,09E-09
MOX2 –3– 0 8,66E-09 8,82E-10
MOX2 –3– 3 2,19E-07 3,99E-09

Table 5. Ratio of neutron activity generated in spontaneous fission reactions and in ( α -n)-
reactions to gamma-activity of heavy nuclides (for ThO2–PaO2–UO2 fuel).

SNF SFn / γ (α − n ) / γ
(Th-Pa-U)O2– 3 – 0 1,56E-14 1,28E-09
(Th-Pa-U)O2– 3 – 3 1,94E-13 2,82E-08
(Th-Pa-U)O2– 30 – 0 5,13E-10 2,08E-10
(Th-Pa-U)O2– 30 – 10 3,62E-08 2,78E-08

It is seen from Tables 4-5 that neutron activity of heavy nuclides is quite insignificant as
compared with their gamma-activity. Fission products also give a significant contribution to total
gamma-activity of SNF. However, as it will be shown below, when spent FAs are placed into the
transport container (TC) described in Ref. 1, radiation situation around the container is determined
both by neutrons and by gamma-rays. Outside of TC shielding, neutron- and gamma-components of
radiation dose are comparable each other. The point is the TC shielding under analysis consists of
steel only, protective layers of light materials are absent. Dominant fraction of gamma-rays emitted by
SNF (from 90% to 99%) is low-energy gamma-rays (up to several hundred of kilo-electronvolts)
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which are absorbed effectively by steel shielding. Neutrons have an energy larger by an order of
magnitude and larger penetrability. All these circumstances plus absence of neutron moderators and
absorbers in the TC shielding lead to the fact that probability for neutrons to go out the TC is higher
substantially than that for gamma-rays. So, despite gamma-activity is more intense (by 8-10 orders of
magnitude) than neutron activity, after penetration through the TC shielding, contributions of gamma-
rays and neutrons to dose rate are comparable each other.

It is shown in the Tables above, what heavy nuclides give a main contributions to total SNF
activity (the same nuclides are the main contributors to dose parameters). It is evident the
computational errors in concentrations of these nuclides affect substantially the anticipated dose
parameters of SNF. It would be reasonable to expect that accuracy of concentrations and doses
determination by the computer code package SCALE is sufficiently high because this computer code
is specially recommended for solving such kind of problems for VVER-type reactors. However, the
calculated concentrations of heavy nuclides are compared with benchmark data for traditional UOX-
fuel. The results obtained in such a comparison enabled us to make the following conclusions:
1. Concentrations of those isotopes which are the main contributors to NF criticality are in good
agreement with benchmark data. For example, discrepancy of U235 concentrations was below
0,4%.
2. For concentrations of those isotopes which are not the main contributors to NF criticality we
did not find a reliable benchmark problem. So, values of these concentrations are taken from
Ref. 4. Significant discrepancies in concentrations are revealed for a series of such isotopes
(see Table 6). Therefore, it may be recommended to carry out high-precision calculations with
aim to determine accurate concentrations of these isotopes in SNF and, thus, to reduce errors
in values of SNF activity and dose parameters.

Table 6. Heavy nuclides with significant discrepancies in values of their concentrations.

Isotope Pu238 Am241 Cm242 Cm244

Error, % 64,9 20,5 13,7 -15,3

The following intermediate conclusions can be made from the obtained results:

1. For both types of neutron radiation, it is possible to form the isotopic groups which meet the
requirements 1-5 during full cooling time for all SNF types under analysis.

2. For gamma-radiation, it is possible to form the isotopic groups which meet the requirements
1-5 but not for full cooling time. There is a time interval at the beginning of cooling time
when these requirements are not satisfied. This time interval is defined by decay rate of short-
lived isotopes. It is true for all SNF types under analysis.

3. Supposedly, this model can work in full scale in several weeks or months after cooling time
period begins. As for neutron radiation, this model can work properly just after the reactor
shutdown.

4. For uranium and uranium-plutonium NF, it is observed significant growth of NF activity for
all three components with every next recycle.

5. Significant errors are observed in concentrations of those isotopes which are not the main
contributors to the reactor criticality but which are able to affect SNF activity substantially.
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Similar isotopic groups can be used in studies on SNF activity sources required for validation and
verification of different computer codes.

Fission products - main contributors to SNF gamma-activity

As it was noted above, SNF activity is determined by heavy nuclides and fission products (FP).
For all SNF types under analysis, contributions of gamma-active FP are calculated. For traditional
UOX-fuel, the obtained results are compared with the data published in Ref. 4.

As a result of this comparison, we concluded that, in contrast to heavy nuclides, FP activities are
calculated with very high accuracy for all significant isotopes (errors - 2-3%). High accuracy of these
calculations is of small wonder because FP generation is mainly defined fuel burn-up, FP yield per
one fission reaction and natural decay rate. These parameters are known with good accuracy.

Also, the anticipated conclusion is made that, for initial interval of SNF cooling time, it is
impossible to select a few FP for correct description of radiation background. This fact may be
explained by large number of short-lived FP. However, for 3-year cooling time, a set of 10 the most
active FP contributes from 97% to 99% to total FP activity for all SNF types under analysis. It is
interesting that set of the most active FP does not change almost for all SNF types but their
contributions do change. The FP set involves the well-known isotopes: Cs137, Cs134, Rh106, Ru106, Y90,
Sr90. If cooling time is prolonged, then a tendency appears to decreasing the number of significant
radionuclides.

The calculated FP activities are collected, for convenience, together with gamma-activities of
heavy nuclides (HN) in one Table 7. It is seen that, for traditional UOX-fuel, gamma-activity of FP is
several times higher than that of heavy nuclides. Activity ratio FP-to-HN increases for longer cooling
times. For MOX-fuel these activities are comparable each other for different number of recycles, and
FP-to-HN activity ratio decreases with time. For fuel composition ThO2–PaO2–UO2, FP-to-HN
activity ratio depends significantly on value of fuel burn-up.

Table 7. Gamma-activities of light and heavy nuclides per one FA.

NF FP, Ci HN, Ci FP/HN activity ratio

UO2-3-0* 8,89E+7 2,31E+7 3,85
UO2-3-3 4,19E+5 6,67E+4 6,28
MOX-3-0 8,59E+7 2,19E+7 3,92
MOX-3-3 4,18E+5 4,03E+5 1,04
MOX2-3-0 8,53E+7 2,37E+7 3,60
MOX2-3-3 4,18E+5 4,47E+5 0,94
Th-Pa-U-3-0 7,03E+7 2,15E+7 3,27
Th-Pa-U-3-3 3,82E+5 1,69E+6 0,23
Th-Pa-U-30-0 9,34E+7 3,01E+7 3,10
Th-Pa-U-30-10 1,36E+6 7,86E+4 17,30
* - 3 years - irradiation time in VVER, 0 years – cooling time.

Dose rate from SNF containers

Further, dosimetric parameters of SNF containers are analysed. It is considered a steel container
(thickness of steel wall - 40 cm) with six FA inside [1]. Parameters of VVER-1000 [6] reactor are
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used in all calculations. A value to be determined is a dose rate (mrem/h) from SNF container for
gamma- and neutron radiation separately. The dose rates are calculated for surface of SNF container
and for 2 m-distance from surface of SNF container.
Information about dosimetric characteristics is presented in graphic form. Variation of dose rate
from SNF container (six FA inside) after irradiation time is shown by the solid line. The dotted line
connects values of dose rate prior to irradiation and just after irradiation under the same conditions.

0 2 4 6 8 10
10
2
10
8
Dos e r ate, mrem/h

1
10 6

3
4
0
10
2
2

1
-1
10 0
0 2 4 6 8 10 12
t, years

Fig. 1. Dose rate of gamma-radiation from 1)UO2; 2)MOX; 3)MOX2.

0 2 4 6 8 10
500 10

3 4
400 5 8
2
Dos e r ate, mr em/h

300 6
1

200 4

100 2

0 0
0 5 10 15 20 25 30 35 40
t, years

Fig. 2. Dose rate of gamma-radiation from ThO2–PaO2–UO2 fuel for different irradiation time:
1)3-year; 2)5-year; 3)10-year; 4)20-year; 5)30-year.
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0 2 4 6 8 10
10
3
10 3
2 8
10 2
Dos e rate, mrem/h

1
10 6
1
0
10
4
-1
10
2
-2
10

0
0 2 4 6 8 10 12
t, years

Fig. 3. Dose rate of neutron radiation from 1)UO2; 2)MOX; 3)MOX2.

0 2 4 6 8 10
500 10

3
400 2 8
Dos e rate, mrem/h

1
300 6

4
200 4

100 5 2

0 0
0 5 10 15 20 25 30 35 40
t, years

Fig. 4. Dose rate of neutron radiation from ThO2–PaO2–UO2 fuel for different irradiation time:
1)3-year; 2)5-year; 3)10-year; 4)20-year; 5)30-year.
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Proceeding from these graphs, the following conclusions can be made:

1. Under transition from UOX to MOX-fuel, dose rate of neutron radiation increases by an order of
magnitude. Maximal growth of dose rate is observed just after irradiation time, dose rate increases
by a factor about 25. For the next recycle, dose rate of neutron radiation increases additionally by
30%. These effects can be explained by relatively high (as compared with UOX-fuel)
accumulation of minor actinides in MOX-fuel. The increased dose rates represent some
difficulties in SNF reprocessing for multiple (more than two-fold) utilization. However, it
complicates unauthorized use of SNF also.
2. Under transition from UOX to MOX-fuel and under further recycles, maximal dose rates of
gamma-radiation undergo practically no changes because it mainly defined by FP accumulation
that depends on fuel burn-up, not on fuel composition. However, relaxation of dose rate with
every next recycle is slightly reduced. This can be explained by effect of minor actinides and their
decay products. These effects begin to act not immediately, and they are accompanied by some
variations of FP composition caused by transition from UOX to MOX-fuel.
3. Maximal dose rate of neutron radiation from Th-Pa-U fuel is higher by a factor about 10 than that
from UOX-fuel, and lower by a factor about 2 than that from MOX-fuel. This can be explained by
appropriate variations of minor actinides accumulation (trans-plutonium actinides are not really
accumulated in Th-Pa-U fuel). For fuel burn-up below nominal value, dose rate of neutron
radiation demonstrates a growth tendency. This effect can be regarded as an additional radiation
barrier against unauthorized proliferation of the fuel incompletely burnt-up. For fuel burn-up
close to nominal value, dose rate of neutron radiation rapidly decreases, and dose rates are
comparable with those for traditional UOX-fuel.
4. Maximal dose rate of gamma-radiation from Th-Pa-U fuel (just after irradiation) is higher by a
factor about 3 than that for UOX and MOX-fuel. For all values of fuel burn-up, dose rate of
gamma-radiation sharply decreases after fuel discharge from the reactor core, and this fact can be
explained by decays of short-lived FP. For fuel burn-up below nominal value, dose rate of
gamma-radiation demonstrates a tendency to increase after such a reduction. For fuel burn-up
close to nominal value, dose rate of gamma-radiation continues to relax but with lower speed than
that during initial time interval. After long enough cooling time, dose rate becomes comparable
with the same parameters for MOX-fuel after the third irradiation cycle.

Finally, the following major conclusions can be made:

1. Correct description of SNF radiation and dosimetric properties requires available benchmark data
on contents of heavy nuclides in SNF.
2. ThO2–PaO2–UO2 fuel demonstrates an important feature: internal transmutation of minor
actinides provided the ultra-high fuel burn-up is achieved.

References

1. N.V.Omelchenko, V.I.Savander, A.A.Smirnov, V.S.Kharitonov. Transport containers for

spent fuel assemblies from nuclear reactors of different types. - Moscow, MEPhI, 2001.
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characteristics of the light water reactor core fuelled with (Th+Pa+U)-ceramics (high fuel burn-up via
DUPIC processes application). - Proceeding of the PHYSOR 2002, Seoul, Korea, October 7-10, 2002,
3B-01.
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3. SCALE: A Modular Code System for Performing Standardized Computer Analyses for
Licensing Evaluation, NUGER/CR-0200, Rev. 4 (ORNL/NUGER/CSD-2/R4), Vols. I, II, and III
(draft November 1993). Available from Radiation Shielding Information Center as CCC-545.
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Calculations with SCALE/SAS2H, ORNL/TM-2000/4.